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Sustainable upcycling of spent LiCoO2 to an ultra-stable battery cathode at high voltage

Nature Sustainability volume 6, pages 797–805 (2023)Cite this article

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Abstract

The continued market growth for electric vehicles globally is accelerating the transformational shift to a low-carbon transportation future. However, the sustainability of this transition hinges to a large extent on the management of waste, including end-of-life batteries where strategic elements such as lithium (Li) and cobalt (Co) are present. Different from the existing pyrometallurgical and hydrometallurgical recycling methods that involve heavy energy inputs and the use of hazardous chemicals, here we show a feasible single-step process that not only reclaims lithium cobalt oxide (LiCoO2) from waste Li-ion batteries but also upgrades it to a cathode with enhanced electrochemical properties. Our recycling process is based on a direct reaction between spent LiCoO2 and added mixture of Al2O3, MgO and Li2CO3, during which the Li vacancies aid the diffusion of Al and Mg to yield dual-doped LiCoO2. The upgraded LiCoO2 cathode possesses even better structural stability and sustains 300 cycles retaining 79.7% of its initial capacity at a voltage of 4.6 V. As evidenced by the technoeconomic analysis, the current circularity approach exhibits cost benefits and could catalyse further progress in the upcycling of different materials for batteries.

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Fig. 1: Regeneration of degraded LCO to R-LCO.
Fig. 2: Structural characterization of R-LCO.
Fig. 3: Properties and electrochemical performance of regenerated LCO.
Fig. 4: Electrochemical performance of regenerated LCO.
Fig. 5: Theoretical calculations.
Fig. 6: Technoeconomic analysis.

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Data availability

All data supporting the research in this paper are available in the main text and Supplementary Information, and original data can be obtained through reasonable requests from corresponding authors.

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Acknowledgements

G.Z. appreciates support from the National Key Research and Development Program of China (2019YFA0705700), Joint Funds of the National Natural Science Foundation of China (U21A20174), Guangdong Innovative and Entrepreneurial Research Team Program (2021ZT09L197), Shenzhen Science and Technology Program (KQTD20210811090112002), the Start-up Funds and Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School. G.Z. and J.W. appreciate support from Qinhe Energy Conservation and Environmental Protection Group Co., Ltd (no. QHHB-20210405).

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Author notes

  1. These authors contributed equally: Junxiong Wang, Kai Jia, Jun Ma.

Authors and Affiliations

  1. Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China

    Junxiong Wang, Kai Jia, Jun Ma, Zhaofeng Zhuang, Yun Zhao, Baohua Li & Guangmin Zhou

  2. Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, China

    Junxiong Wang, Kai Jia & Zheng Liang

  3. Faculty of Materials Science and Engineering / Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China

    Hui-Ming Cheng

  4. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, China

    Hui-Ming Cheng

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Contributions

All authors contributed to this work. J.W. completed a major part of the experiments and drafted the original version of the manuscript. K.J. and J.M. helped perform some of the experiments and provided extensive suggestions for revisions of the original manuscript. Z.L., G.Z. and H.-M.C. discussed together and proposed the concepts of this paper and made extensive revisions to the original manuscript. Z.Z., Y.Z. and B.L. assisted in the design of some test methods and materials characterization.

Corresponding authors

Correspondence to Zheng Liang, Guangmin Zhou or Hui-Ming Cheng.

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Nature Sustainability thanks Lei Pan, Gavin Harper, Lianqi Zhang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Wang, J., Jia, K., Ma, J. et al. Sustainable upcycling of spent LiCoO2 to an ultra-stable battery cathode at high voltage. Nat Sustain 6, 797–805 (2023). https://doi.org/10.1038/s41893-023-01094-9

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